Xi Zhang , YouPeng Lu , Meilin Zhu , Caizhu Liu , Zhu Zhu , Qinghong Zeng , Zhuangmei Li , Yuhua Wu , Jianbo Wu , Hui Zhang , Hongcun Bai
{"title":"土壤对Be2+和Cu2+的固定化:俘获行为、定量模型和量子机制","authors":"Xi Zhang , YouPeng Lu , Meilin Zhu , Caizhu Liu , Zhu Zhu , Qinghong Zeng , Zhuangmei Li , Yuhua Wu , Jianbo Wu , Hui Zhang , Hongcun Bai","doi":"10.1016/j.molliq.2025.128620","DOIUrl":null,"url":null,"abstract":"<div><div>Be<sup>2+</sup> and Cu<sup>2+</sup> ions from beryllium copper alloy processing pose significant environmental pollution risks due to their high toxicity. The immobilization of Be<sup>2+</sup> by soil is an important link in understanding its pollution and also a core step in soil remediation after beryllium pollution. However, understanding the immobilization of Be<sup>2+</sup> by soil is insufficient, particularly regarding the influence of soil texture, quantitative adsorption processes, and microscopic interaction mechanisms. This study systematically reveals the macroscopic and microscopic behaviors and mechanisms of Be<sup>2+</sup> and Cu<sup>2+</sup> ions in soils of different textures through batch adsorption experiments, mathematical models, material characterization, and quantum mechanical calculations It establishes a quantitative multi-scale framework addressing these gaps. Key findings include rapid Be<sup>2+</sup> adsorption (about 30 mg/kg within 16 h), distinct pH-dependent patterns, and exothermic reactions. Adsorption kinetics followed the pseudo-second-order model (R<sup>2</sup> > 0.99), while isotherms (Freundlich, Temkin, D-R) confirmed chemisorption dominance on heterogeneous surfaces. Characterization techniques revealed that clayey soils, with larger specific surface areas and active sites (Si<img>O, Al<img>O), facilitate immobilization via chemical bonding. Quantum calculations further confirmed the superior adsorption activity of kaolinite's Al-terminated surface for Be<sup>2+</sup>. This can be evidenced by the shorter Be<img>O bond length (1.589 Å) and larger adsorption energy, rationalizes the higher immobilization strength of Be<sup>2+</sup> observed in experiments. This work provides profound insights into the multi-scale mechanisms of Be<sup>2+</sup> immobilization in soils.</div></div>","PeriodicalId":371,"journal":{"name":"Journal of Molecular Liquids","volume":"437 ","pages":"Article 128620"},"PeriodicalIF":5.2000,"publicationDate":"2025-09-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Immobilization of Be2+ and Cu2+ by soils: Trapping behavior, quantitative model and quantum mechanism\",\"authors\":\"Xi Zhang , YouPeng Lu , Meilin Zhu , Caizhu Liu , Zhu Zhu , Qinghong Zeng , Zhuangmei Li , Yuhua Wu , Jianbo Wu , Hui Zhang , Hongcun Bai\",\"doi\":\"10.1016/j.molliq.2025.128620\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><div>Be<sup>2+</sup> and Cu<sup>2+</sup> ions from beryllium copper alloy processing pose significant environmental pollution risks due to their high toxicity. The immobilization of Be<sup>2+</sup> by soil is an important link in understanding its pollution and also a core step in soil remediation after beryllium pollution. However, understanding the immobilization of Be<sup>2+</sup> by soil is insufficient, particularly regarding the influence of soil texture, quantitative adsorption processes, and microscopic interaction mechanisms. This study systematically reveals the macroscopic and microscopic behaviors and mechanisms of Be<sup>2+</sup> and Cu<sup>2+</sup> ions in soils of different textures through batch adsorption experiments, mathematical models, material characterization, and quantum mechanical calculations It establishes a quantitative multi-scale framework addressing these gaps. Key findings include rapid Be<sup>2+</sup> adsorption (about 30 mg/kg within 16 h), distinct pH-dependent patterns, and exothermic reactions. Adsorption kinetics followed the pseudo-second-order model (R<sup>2</sup> > 0.99), while isotherms (Freundlich, Temkin, D-R) confirmed chemisorption dominance on heterogeneous surfaces. Characterization techniques revealed that clayey soils, with larger specific surface areas and active sites (Si<img>O, Al<img>O), facilitate immobilization via chemical bonding. Quantum calculations further confirmed the superior adsorption activity of kaolinite's Al-terminated surface for Be<sup>2+</sup>. This can be evidenced by the shorter Be<img>O bond length (1.589 Å) and larger adsorption energy, rationalizes the higher immobilization strength of Be<sup>2+</sup> observed in experiments. This work provides profound insights into the multi-scale mechanisms of Be<sup>2+</sup> immobilization in soils.</div></div>\",\"PeriodicalId\":371,\"journal\":{\"name\":\"Journal of Molecular Liquids\",\"volume\":\"437 \",\"pages\":\"Article 128620\"},\"PeriodicalIF\":5.2000,\"publicationDate\":\"2025-09-27\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Journal of Molecular Liquids\",\"FirstCategoryId\":\"92\",\"ListUrlMain\":\"https://www.sciencedirect.com/science/article/pii/S0167732225017970\",\"RegionNum\":2,\"RegionCategory\":\"化学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q2\",\"JCRName\":\"CHEMISTRY, PHYSICAL\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Journal of Molecular Liquids","FirstCategoryId":"92","ListUrlMain":"https://www.sciencedirect.com/science/article/pii/S0167732225017970","RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q2","JCRName":"CHEMISTRY, PHYSICAL","Score":null,"Total":0}
Immobilization of Be2+ and Cu2+ by soils: Trapping behavior, quantitative model and quantum mechanism
Be2+ and Cu2+ ions from beryllium copper alloy processing pose significant environmental pollution risks due to their high toxicity. The immobilization of Be2+ by soil is an important link in understanding its pollution and also a core step in soil remediation after beryllium pollution. However, understanding the immobilization of Be2+ by soil is insufficient, particularly regarding the influence of soil texture, quantitative adsorption processes, and microscopic interaction mechanisms. This study systematically reveals the macroscopic and microscopic behaviors and mechanisms of Be2+ and Cu2+ ions in soils of different textures through batch adsorption experiments, mathematical models, material characterization, and quantum mechanical calculations It establishes a quantitative multi-scale framework addressing these gaps. Key findings include rapid Be2+ adsorption (about 30 mg/kg within 16 h), distinct pH-dependent patterns, and exothermic reactions. Adsorption kinetics followed the pseudo-second-order model (R2 > 0.99), while isotherms (Freundlich, Temkin, D-R) confirmed chemisorption dominance on heterogeneous surfaces. Characterization techniques revealed that clayey soils, with larger specific surface areas and active sites (SiO, AlO), facilitate immobilization via chemical bonding. Quantum calculations further confirmed the superior adsorption activity of kaolinite's Al-terminated surface for Be2+. This can be evidenced by the shorter BeO bond length (1.589 Å) and larger adsorption energy, rationalizes the higher immobilization strength of Be2+ observed in experiments. This work provides profound insights into the multi-scale mechanisms of Be2+ immobilization in soils.
期刊介绍:
The journal includes papers in the following areas:
– Simple organic liquids and mixtures
– Ionic liquids
– Surfactant solutions (including micelles and vesicles) and liquid interfaces
– Colloidal solutions and nanoparticles
– Thermotropic and lyotropic liquid crystals
– Ferrofluids
– Water, aqueous solutions and other hydrogen-bonded liquids
– Lubricants, polymer solutions and melts
– Molten metals and salts
– Phase transitions and critical phenomena in liquids and confined fluids
– Self assembly in complex liquids.– Biomolecules in solution
The emphasis is on the molecular (or microscopic) understanding of particular liquids or liquid systems, especially concerning structure, dynamics and intermolecular forces. The experimental techniques used may include:
– Conventional spectroscopy (mid-IR and far-IR, Raman, NMR, etc.)
– Non-linear optics and time resolved spectroscopy (psec, fsec, asec, ISRS, etc.)
– Light scattering (Rayleigh, Brillouin, PCS, etc.)
– Dielectric relaxation
– X-ray and neutron scattering and diffraction.
Experimental studies, computer simulations (MD or MC) and analytical theory will be considered for publication; papers just reporting experimental results that do not contribute to the understanding of the fundamentals of molecular and ionic liquids will not be accepted. Only papers of a non-routine nature and advancing the field will be considered for publication.